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Title: Probing autoionizing states of molecular oxygen with XUV transient absorption: Electronic-symmetry-dependent line shapes and laser-induced modifications

In this paper, we used extreme ultraviolet (XUV) transient absorption spectroscopy to study the autoionizing Rydberg states of oxygen in an electronically- and vibrationally-resolved fashion. XUV pulse initiates molecular polarization and near-infrared pulse perturbs its evolution. Transient absorption spectra show positive optical-density (OD) change in the case of $$ns{{\sigma}}_{g}$$ and $$nd{{\pi}}_{g}$$ autoionizing states of oxygen and negative OD change for $$nd{{\sigma}}_{g}$$ states. Multiconfiguration time-dependent Hartree-Fock (MCTDHF) calculations are used to simulate the transient absorption and the resulting spectra and temporal evolution agree with experimental observations. We model the effect of near-infrared perturbation on molecular polarization and find that the laser-induced phase-shift model agrees with the experimental and MCTDHF results, while the laser-induced attenuation model does not. Finally, we relate the electronic-state-symmetry-dependent sign of the OD change to the Fano parameters of the static absorption line shapes.
 [1] ;  [2] ;  [2] ;  [2] ;  [3] ;  [4] ;  [1]
  1. Univ. of Arizona, Tucson, AZ (United States). College of Optical Sciences. Dept. of Physics
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  3. Texas A & M Univ., College Station, TX (United States). Chemistry Dept.
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of California, Davis, CA (United States). Dept. of Chemistry
Publication Date:
Grant/Contract Number:
AC02-05CH11231; SC0012198; W911NF-14-1-0383
Accepted Manuscript
Journal Name:
Physical Review A
Additional Journal Information:
Journal Volume: 95; Journal Issue: 4; Journal ID: ISSN 2469-9926
American Physical Society (APS)
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Texas A & M Univ., College Station, TX (United States); Univ. of Arizona, Tucson, AZ (United States); Univ. of California, Davis, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Army Research Lab. (ARL) (United States); US Army Research Office (ARO)
Country of Publication:
United States
74 ATOMIC AND MOLECULAR PHYSICS; atomic & molecular processes in external fields; interatomic & molecular potentials; multiphoton or tunneling ionization & excitation; optical transient phenomena; strong-field-induced spectra; ultrashort pulses; molecules; Rydberg atoms & molecules; attosecond laser irradiation; attosecond laser spectroscopy; configuration interaction; dipole approximation; femtosecond laser irradiation; femtosecond laser spectroscopy; femtosecond pump-probe transient absorption; first-principles calculations; Hartree-Fock methods; high-harmonic generation; photoexcitation; Schroedinger equation; ultrafast pump-probe spectroscopy
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1353276